Formation of Graphene Nanoscrolls and Their Electronic Structures Based on Ab Initio Calculations

Rolling up two-dimensional (2D) materials can formquasi-one-dimensional nanoscrolls, which are expected to have novelproperties due to their larger space of structural parameters. In thisLetter, the structural dependence of formation energy wasinvestigated based on more than 90 different graphene nanoscrolls(GNSs) throughab initiocalculations. A quantified relationshipbetween formation energy and structural parameters is discovered,which could provide universal description of rolling up 2D materialsbeyond graphene. Further calculations on electronic structures showthe opening of bandgap in GNSs with ultrahigh carrier mobilities upto 107cm2V-1s-1. The structural stability under room temperaturewas also testified by using molecular dynamic simulations. This workprovides general insights into the rolling-up strategy and demon-strates the tunable properties of GNSs, thus extending the scope ofthe researchfield for 2D materials.